Molten-bath process for fixing nitrogen and means for effecting the same.



G THE SAM.

Patented Mar. 7, 1916.

` 1. E. BUCHER. MOL'EN BATH PROCESS FOR FIXING NITROGEN AND MEANS FOR EFFECTIN APPLICATION FILED )CT. l9,ll9l4.

- 5mm@ STATES PATENT orricn.

JDHN E. BCHER, F COVEltTTl/Y, RHODE ISLAND, 'ASSIGNOB TO NITROGEN PRODUCTS courrant?, orfrnovmnucn, nnonn IsLANn, n conronnrron or :more ISLAND.

riemen-BATH rnocnss ron rrxING aangaan x y ToaZZ whomyt may concern:

Be it known that I, JOHN E. Buenas, `a citizen of the United States, residing at qGofventry, inthe countyof Kent and State y ""ofRhode Island, have invented certain new 'f yandznscful Improvements in Molten-Bath fPrcessesyfor Fixing `Nitrogen and `Means n `forfEifecting Same, of which the following yisagspecication. 1 l

@En :my Patent No.11,091,425," granted MarchgQfl, 1914, I` described` with 'particuarity a nitrogenfixing process in the effectutionofwhich a gcatalyzer, e. g. iron, .was

used preferably solid "and i finely divided form., Herein cre wasv exercised to `avoid levating the'temperature ofthe reactive' ssiabove"thereutectic pointof the carbon containing'4 catalyzer, in i orderfto preserve onfbeing specially]` active andhence able orniingreaction at even moderate temperagradually` elevated to the said eutectic oint, the? reaction becomes increasingly ligorous'; but when the finely divided cata- `11i.yzerhsinters orrlmelts the requisite contact t, n conditions are disturbed and the process be- )Sucomes correspondingly'more or lessineffeci tive".4 havebeenavvare forra `long time `that such 1a catalytic material as molten iron, 3 evian at temperatures above 1700o or 1800 G.

` "5911 PI'PGGSSU` offrand `means for fixing nitrogen aange the instrumentality @finden @er y bon` digs'glving'catalytic `material and has "beforinedlg y ,n

` havefalso aune Wat-edf with turbo;1,1%.`

t Specification of Letters Patent.

arv very-f great^ catalytic f surface `containing ,carbonin solution therein the `rhssolved car-4 o* Participate`k la cyanogen y compoundr s. vAsthetemperature of such afmasjs would be; available` for use in the process, y "but, the problem vvas to so handle such a i 4* ll f `Ina-terial,inconjunction with other elements, i i 1 asto restablishthe conditions under whichv ",cyanidy'forniation could again 1 occur copi# The l present invention' therefore relates to nrrnoenn Ann Manns ron rrrnc'rnfrel THE sans. l

Patented Mar. 7, 1916.

l Application filed October 19, 1914.` Serial No. 867,374.

These and other. objects of my invention I 'to a converter yin construction, and comprises a receptacle 1, of cast iron or the like, suit-l `ably lined, as at 2, and provided with twyers or small diametered openings 3, preferably in the bottom lining thereof, through which the gaseous reagent `(bubbles of which have been designated 4) 'may be assed into the molten iron or like catalytic material, Within the furnace.

The gaseous reagent is supplied to the `tvvyers through a conduity 6, and an electrode 7 of graphite or the like is projected, through a conduit like opening 8 near the furnace bottom, into contact with said moltencatalyzer. The electrode 7 may besuitably packed, as at 9, to prevent the vescape of the molten material, and has connected thereto a bus bar or lead 10 from a source i of electric current, preferably of relatively low voltage (20 to 25 volts) and large amperage. The electrode 7 may also serve asa tap for the molten iron or the like, if desired.

'Throughone side ofthe .casing 1 extends a conduit 11 for'the introduction of graphite, or a like preferably ash-free carbonaceous material, into the electric furnace; a screw conveyerl 12-serving`to `propel the graphite through the passage. p

Upon the opposite side is shown a confduit 13 for the escape of the gaseous and "vaporous reaction products which are, of

course, to be collected. y y v The furnace is provided,withA a cap 14 lof suitable non-conductive material, such as will be hereinafter referredto `in connection with-the furnace lining? This cap maybe connegtfed to anfiron backingy plate 15 and mayinyfact bcniolded thereupon. Through the cap extends `an electrode: supporting bar 16 of `which may havetherearound pro swf-17 of heat insulating material.

'i .'eiitremity' ef thi-saber may li'eprei rests 1 upon .the interiorly threaded upper electrode 1 9into -Whiehbar 16 is screwed; f the '.'Cap' l8 'being of material similar "to lthe manner 1110W to be'described a. this' upper electrode also, preferably,

Above the VAmolteni mass 5, 'is shovvna Cha'ige'Ql kof' J graphite or. other suitable car`A ,molteniromas -g1`6z1'tfimportance as by reason thereof, a fnuiniberfof v important results are attainech Vv` Inyfthe. first place it keeps the iron .or its f b'on throughout the bulk thereofat all times.; l fflheJpresenee off-the smallcarbon masses ithr'oughout'a large `part of theniolten c ataij e ly'zercausesrthe larger' bubbles yof the gasef` ousf?"L reagent fused',

" contact with. the yiron a sufficient `length of time to'enable. the gases toeiiiciently ticipate.- inthereaction.r By distributing the; y gaslforfgasesthroughout l `V`al soi establishes,the requisite extent of cata# lytic ,1 solution surface g. "since, ,of course, -v Wheinever albubble of, forexarnple', mixed "itrbgen and sodiuml vapor! ispresent .in vthe Y iq'uid,v such a surface is .temporarily estab-,` ylished all, around the bubble, land the smallerf;

thesereeateSurface-r l A'account ofthe `operating temperaturef beingrrelatively high," as'compi'red With, .forjy example, ythe redV4 heat preferably used vWhelagbe 'so yextensive as. that, required for the processWhenusing a' solid catalyzer; lt, nevertheless," the Amore extensive. this surf-. ece,l .f even Whenmolte'n, the more efficient the? z is'sojciated carbony masses in the .'m'elt j. AnotherA advantage 1 arising vvfrom this". dis-f. f plosltionlqof the ycarbon l1H. @n electricfurnace' urface l of Ithe molten catalyzer, on is'v of course in most intimate h theiron or the like, may bef .teete'd as'rshownbyan electrode cap 18v which j lining. Ay pack-mgQO 'of kieselguhr or "the` be `used to= seal the openingin thel cap21 servingto keep this pacli-y kring. vinplace when the electrode is being ele-y attached to the eye The rod 16 may "als' o be weighted,` as'at 23 to insure" the 'gproper'settlingofthe electrode l8,fi'n the f y being yof graphite andfhe'nce not'being particularly weighty.. f

,bonaceous material and Whenthe weighted ele'etrode 19, whiohjis relatively quitev large .'infTeross-section as compared to. that of the.

` is allowed to'deseend, 'it

' y mill and the Y particles andfo'rcesja large vrpfortio`r 1. ,thereofdeeply-'into the bulk.. of shown. `This feature is of y powder makes the mixture equivalent practically saturated .with carr` afterl it -hasbeen suiic'iently'imoistened.sandv l1t can bevfheated dir etlyfin l l `Without .dlsintegr'ating'.` 1nfact it-becomes vto .break up into y very.' ,ly small ones andfurtherholdsthe reagent in` .fb

are.. 4 While further,nearly,allfofgthehe'at ,is genl the vliquid mass'it L erated in the resistor between the. upperv 105 atalyzer` isfain the,'solidphase,fthef molten f catalytic 'solutionsurface need .not

prob sfghenceanother value of the'. `smal-l y'to liquidafterz passing I .vvithlsuitable linings', by vthe r'nean's'" 'herein after -indicated'fitfi's i possible-to., n as usedA asian internal 'resistor in .theifurnace 'y wherebyto'introducel heat vdirectly in contact with. the riron `and so v ayoid the zdisadv y.vantagee of theflexlceedingly high temperature ofthe electric. are togetherpvvith the at` ,f tendantdiihcultiesof' currentl and'heat regu-- lation' and distribution.,` The'. graphite yparf ticles` are preferably between three and twenty mesh.

Beforediscussngthe prebess further, the 75 lining of the furnace,f'shofuld` beconsidered f since many commonly usedzlinings' are lnot.4

afable 'for Se with the'proces. Accord; 1 'ingly the linings? aferfereredqas follows? The veryrhard compact magnesi brick, Such .as is used inv open hearthffurnaceais pow-- dered rin an viron mortar sojthat it vmay r.be kpassed through aftwe'nty mesh'sevejf'lo z fty parts ofthisypowdefl`-add 'fifty parte.. fof alundumv cement 'jandffromftvvo tqffive l85 l parts of boraxglassor borazzr."4 4v'lhese mate- .'rials maybemixedlandground in. a suitable proportions kmay beLvaried quite.. Widely. The .above .proportions were, .how-f rever,'. those `first1 used: @Withjfalliali ,metal vapor'and nitrogen and gave such good .results that they Werealvvays used. thereafter; The coarse i magnesia brick -l 'i porous that 95 stillisrsoapoi Jus that the blast flame Pamped verrerie-it like rock, when heated .bythe electric are.; kllowever,v the' :effective .foontacu establishedgfloo etwe'en the' graphite; 1 particles themselves y'and between., Said-.particlesand the upper electrode lpsubstantially -jp'revents 'arcin'g,

electrode andthe molten iron. 'v ils-'the latter 4is'an excellentconductor the-heat travels f downwardly krapidly softhat l the"icyanogenv compound forming e reaction begins to occur f the/instant that-*the bubbles Y are :formed "at "110 the twyers. The furnacej'is preferably in-` 5 Sula-ted, especially -atryltheibottom;' and lif the temperature becomes too high at any g time, the current y.may'beA shut offy entirely for a-few minutes.

The :gf-@ousv reagent .employed is.v prefer@ ably.;y a mixture jef salkalijmetal" v aporland nitrogen; these gases Abeingp'preh cated "to'atl-.fl i

and'fit may be.y read 4.yan-id formei'by 12o i ysodimm vbe used,y there may' be 1 an, jjexess fof.' I

l A ample, insteadof sodium.

brother suitable alkali compounds, `for ex- (1)1lNazcoaticafu@auaomacofisasob cfurisl The soda ash may be introduced as liquid X "orvapor,or it, as Well as suitable alkaline r `deter "gas "11,0: The soda` ashcan` also becaused to .yield odilun by carrying` it through a` carbon reerated asperthe` equation 1 (2) Naomi-zogenaamd j il sistem"lesignated` 9,5;` the sodium being 1 The resistor is contained in a suitablereeeptacle4 2e, havmlgltherein an inner lining 27; similar to that designated 2; kieselguhr l j 4or poivderedmagnesia "28` being` interposed ibetweenthe innerfliningand the iron shell l flttofprotect thelatterfrom the hotsoda ash andfaljso to conserve heat,y `I find that it is advisabletoythusprotect iron parts of the apparatusl Wherever` said parts may `be subt i jectedjto: s ucha temperature asis required tovlvolatillze soda ash.' Where, however,4

lkali:metal-is`` delivered, assuch,` in either l liquidkorfvaporeus condition to the charge, ,t thefintermediate,kieselguhr or other `refractoryforbasicrliningis not absolutely neces-l sary; butis preferably used, as shownfat L28.

fTliisiloose graphite` coke, or other suitable `cabonaceous secondary resistor is 1n `contacta iheiboaom thereof with a graphite t l, electrode 29 tovvhich is connected the negaf` tive busbarorilead 30 of this portion ofthe apparatusA A similar electrode 31 lcontacts rentlto `electrodeBl `and the resistor 25 may t, be'" thereby heated to incandescence.

p rlmizrture of, forexample, soda-ashand i nfrgenymayv "be sled into 4the `reslstor l l the@resistor` to `emerge Ytherefrom as sodium through conduit 34 and descends through yvlapor` and carbon monoXid.

course depend upon` the teme tapfer-emblem effect' it'l'as any. as ps- `n yorder "to supply f the metallic vapor I of, or?`eir`av1riple, sodiumginstead of the less Yapoiizable`s0`da ash, to the (molten` cataly- L"exothermicllbecause oi the free metal vapor.

l i M Thejlcoke, ori-itsequivalent,'forthe secondsister mayubesupplied in anysuitable i `with thetopof thereslstor and mayV extend I up `through a cap and packing 32 as in ,thel

caseffofthe stem 16,1" ofi electrode 19; The

n 24 positive bus bar Ssupplies low voltage cur- Acormpletely this reaction takes l eactionf infthe; molten ironwill become formt Further, Whether the soda ash, for

example, be treated directly in the secondary resistor `S25 or in the bath heated by the primary resistor 24, in either case, the great quantity of heat required when such. a material is used is economically furnished and the production of the nitrogen compound i sought is facilitated. This product is preferably, but of course not` necessarily, cyanid; since if insuiicient carbon be supplied to the reaction zone of the furnace proper, cyanamid will be formed. The carbon for this zone, While preferably obtained from the graphite `masswhich constitutes the primary electrode When the operation is 35 conducted in the manner above described, may also be Vblown in with the gaseous reagentor be otherwise added in the vform of fuel oil, a's by means of the nozzle 36. In 1 any case, it is preferably ash-free as4 the 90 accummulation of ash in the furnace is objectionable, since Whiley the iron, manganese,

oxygen, sulfur, phosphorous or alkali metals `base of the cyanogen compound to be formed, the operation may be continued for a long time until the lower linings have 'to be renewed. The 'e linings, I may here state, can; be healed strongly While still moist and so'far not one lining-has shown l a crack or break after repeated usage;

While in one "of the earlier experimentsa cast iron. pot used inlieu of a furnace was partly melted vfrom the outslde of the stovelike `refractory liningivithout injuring the latter which was used successfully in a subsequent run.

I havementioned above the possibility ofv 120 vlowering'fthe temperature of the bath or melt and this may be done by usinga mix,- ture of catalyzers, iron of course belng but `one of the carbon dissolving substances available. Thus v a ferro-manganese bath,

` especiallyV if potassium be used in lieu of sodium, will permit of operating the process `at a temperature which would not be effective when the catalyzer is iron, alone, and

`the cyanogen basef metal, sodium. Nickel Tend.

A'iron at 150()o more graphing ix-borethe liquidalevely l eated`v sodium-nitrogen vapork bubbles up :through tlie `molten catalyze; the carbon in solllution 'the-latter y(the ndition) unites with the alkali metal i andv with the nitrogen to et, once form oyanid svntlietically 'according rto the 'eq 11a ti0`n:l

(4) "Nsafl-C-INASQNaON-" 200 caloresl Thefcyanid distils out rapidly :mdf there? after condeuses1en`sily f f 'liigher'f temperatl'ne; than I have indiczited JK"zmfdj,`in f`fac't Ii `lieve successfully' produced cyid y in l"the manner just described? by figgjelectric arci-VIy hence do not desire ltolfbe Y linii'tedito ny particularr temperature `but `V4'eite'rate,that the process is operative oyei-` Le. verylconsiderable rangeof temperature,

gfzibleeatalyzer or catalytic mixture Willbe` infother thanthe solid pha'sefand tlieupper linitfbeing the 'temperature at which -tlie reversible reactionjtends to` cause thefdis-4 *.fsfciition, of cyanid rate substantially equelto 'that at which used the" term' vapor-iles e; generic expresimmple, as lsodium- "Vapor, end -vvoletilized,

sodium carbonate orthellikef In either-'casel itff-r willbe understood that such vapor sjjisr fsdzipted to, supply -a,` metal ycapablev of be- Coming the bese of it cynogen compound'to thereof, is. cons"id'erbly eboyeth'git df the ytmsplielz The.` .gases '1 mi@ 1j, hence compressedgnd tli number otmolecules l 'nitrogen ndgffor' example, sodiur'n` per, unit of =fvolume isicoriespondingly rester, which obviously 'tends "to, intensifyt ej' reaction.

HYig-'ftliiisdesoribed my invention what' :claimjixs: flfhefEA ,process'of 'operai-,ulg fari.k ,electricl i ce"tolixv'nitrogenftherein which con f vfL tzigec'iusly'padded; to `the bath to .this saunev s ;Refe'rring'now tothe dramingend,assum-y ngthatthe molten'` catalytic materielV Abe A' l C.,' and'sth'at graphite particles aye beenforced deeplythereinto v vfhilefstilly rests upon 'the moltenv iron 1'*7 then when the pre"` molecules :of ich @are epperentlyy iny peculiarly active `The operationfrnay ybe, conducted'y e 1 the lower limit-being that at which noeveil;

y i it Iis formed I ncertainfof-the appended claims I have ioii togcov'er botligaseous metal, such,1fo`r y l.the extent of thecmfbonlsurfaice thereof pre- 1 sented ,to said bath,

"metal end free nitrogen `to`-fo`rm a, compound of seid zilkahmetall.;r s

prises subjectingI e mass of v molten .cabof dissolving,`r catalyzer" contained' in seid fuir-.2 nec`e'to the action offfr'ee nitrogen and Kuper 'adapted to' supplyffthe base of a ogen compoundr to beformfed said molten` m cntalyzer to combine y:carbondissolvedini the flatterv directly wi'tlr saidl nitrogen and f base, While constantly renewing ,the carbon content of'the catilyz'er yfrom carbon, parti-' A'cles pressedv doWirntotlie' interior of said ymass in partat least-,bythe weight of'excess carbon 'floating upon )seid .catzil'yzeg and supplying vheat rto saidfurnece by passing an 'electric current "of higlr density throughl said iotingcarbomg i "f "f 2.y The process llo f operating "an electric v furnace 5to kfix vnitrogentherein?which comv y prises `s"u jecti'ng ifr mess-fof -fmolten carbon' dissolving y catnlyzer. Contained vin" said fur nace, tothe action'ofjefree nitrogenfand a vapor adapted tof-supply tlie-llmli -inetal base of e cyanogenv compound/to 'be formed" in seid molten catalyzer; to combinecarbon 'dissolved in the letterldirectly with said ynitrogen and alkali. metzilfbase, While constantlyrenewingthe',fcnrboncontent of the. catalyzer. from `carbon"...particles ypressed downinto y the interior of said.r mass in part et leest by, thefweiglit of excess" carbon'foting upon yseid. 'catalyzerg 'and supplying heat to said -furnace by passing an e ectric curf rent kofliigsgfli densitythrough seid floating carbon.; 4 y ,f f f' lQfTlie' process of' operating mi electric furnace `to fix niti'ogextherein Wliioli compriseselcotricallyhezitinzgj:tl cari-bon resistor' in jsaid,'furnace whileseid`v` esistoiyv is fiort'ting upon zt bath of-carbon dissol materiel, seid resisto'ri'lmving v'theosu onthe'reof in ,fragmentary 'condition to' increase andy 'reacting rupon the carbon dissolved from'isaid'resistor by; said y :catalytic I rmtleriitl,y Wi th7{elkali rmetel and- 'f free nitrogen to formaztfcyan'o'vg'en' compound of said alkali metelgy 4. The process yof.operzuingf au 'electric ilpperntus to `fixynitrogen thereinwhich compriseselectrically heatinggmal cmfoion resistor y I.111 :i part ot sind' 'epparatus yWhile said re- 115 :.sistor `is. floating 'upon' al moltenfbe'th 'of carj f bon* dissolving catalytic niaterinl; andv reactsv ing upon: the carbon dissolyed from saide sistoibysaid catelyticmeteriel, with alkali cyanogen 5; process oioperetingzin electric f f apparatus yto lixfnitrogentherin' which comprisesl electiically.lieitingw` lagprir'nary andl u' secondary c carbon resistor v kand.treating the secondiry resistor` with ai, compound adeptedto reactfwithfthecerbonxthereofztolibere ,-,gite :t metalfcapnble of aetingais'ftlie basezof" gectinge portion ofthe primary' resistor to Ying cateltic y j` with carbon, to contact `with a vapor aapted'to supply the "base of a cyanogen com-` pound to be formed, simultaneously causing nitrogen to contact with said catalytic` `material to directly combine the carbon (iis` `solved therein with said metalrand` nitro-` gen to form said cyaiiogen compound, and ,f substantially,-` simultaneously resaturating`y with carbonjthe catalytic Vmaterial from which the dissolved carbon has been so rei posed deep in the interior of said mass.

a 12. The process ofxinglnitrogen which coniprisessubjecting a mass of carbon dis- :solving catalytic material While in the molten state and `substantially saturated with car- ;Nbomto contact throughout the'bu'lk of `said 11:mass, `Witla a vapor adaptedfto supply a "metalcapable yofV becoming the base" of a i cyanogen compound to bel formed, and s- `miilioneously causing nitrogen to cont-act i'nlike manner with said catalytic material `-tot directlygfcombine `the `carbon dissolved therein "with `said metal and nitrogen to "fomsaidlcyanogen,compound. 13`. The process of fxingnitrogen which consists in causing 'gaseous material, com- ;fprising nitrogen angl a vapor adapted to `act` as thersource of a cyanogen compound "base, to bubble through a'molten bath oi"` carbon ,dissolving catalytic'material which.` L issubstantially saturated Witbcarbon, While li ofifinelyfiivided carbon capable of break# i ingup the bubbles ot' said gaseous material inoo bubbles of materially `smaller size." l `ivlaereby to increase tbe extent ci? molten metal surface in Contact with said gaseous i mterialfancl maintain said bubbles "195 `cous material; 'in contact with. said catalytic i material for an increasecltime. y L 14. The process of' fixing nitrogen which gcomprises subjecting anlass of carbony disi i and substantially satiiratedrs'fith caffiifirix` to@ "Contact with: bubbles eomprlsmgja mi irre i Mmetalconstituting which is capabledof' 111g as the base of a cyanogen compound L" solving rriaterlalQ` while in the molten ,state fi i contact "with )bubbles comprising a` mixture f oflfree nitrogenfand a metallic vapor the "rnetal fconstitliting which isjcaiiable oit' acti th ngias thefbse of a', cyanogreli` compoundgfut 1 ew free nitrogen and `a metallic vapoiztlie comprises subjecting; a; mass of carbon lis` i moved," at a large number of points dis-` prcssingdeep down intorsaifl bath, `a mass solvmgmaterial, 'While in the moltenstalte i i and substantially saturated with carbon, to

fornzied;l to directly 'combiiie the corbeil' 13%:

i and -1 comprises establishing extended., mobile .fn'ljolten carbon dissolving materiali at'fwliicli I saidv mass,v under pressurej anda vapoijadapted to supply the 'baseofA said lcyanogen confipoiinda and simultanesolvedinsaid material at said surfaces; with genfcompound. {1 7.' Theprocessof fixing nitrogen kWh-ich f com cata ytic solution surfaces in a massv of molten carbon? dissolving material, atwhich surfaces a cyanogen compound itcirining re-L raction'mayloe effected, by injecting into l f 2151' said mass;

' vapor adapted tosupply the hase'fof said if said ymaterial fat vsaid surfaces', .with said tent of said surfaces.

` jstantly', moving catalytic soluton'surfaees terial', at which surfaces a 'cyanogen'v cour L 49 pound forming reaction f 'y injecting into said mass,

vfree nitrogen and lalkali nietaL' and simultaneously reacting upon molecules of carbon kydissolved in said material at said surfaces,

45 yWithfsaid nitrogen and alkali metal. f,

51@ '19. An electric. 'nitrogen fixing furnace if comprising afinass of molten catalytic carbondissolvingmaterial, a resistor adapted f s to supply carbon to said material andfrloats molten. inaterijalto cause said metal and l carbonfdissolved" in said catalytic material.y

` 1f eoinprisinga massl of molten catalyticcar# f i bon 'dissolving material,v a resistor adapted tact therewith/and means for introducing 'diseased ia Said mass with ,said niemand 1 nitrogen` to form said cyanogen compound,y retarling the' .emergence oit said bub- `bles `fiom. the niolteii material to prolong f 1 6. The process of fixing nitrogenfwhichcatalytic solution surfaces in ,a mass of surfaces a Acyanogen compound forming re faction Amay (effected,l by injecting into free] nitrogen ously reacting upon molecules of'carboii dissaidnitrog naiidfvapo'r torform saidcyanorises @establishing i extended mobile` under`-vpressure', free nitrogen and",-

cyanogen compound, s iiriultaneouslyjieactf y'3 ing upon molecules k of Vcarbon dissolvecl'in5 vnitrogen and .vapor tofform said cyanogen compound, and so {retarding the .upward n passage through said mass of said nitrogen a aiidjvapor as 'to increase the aggregate ex-y p f i8. The processl of fixing nitrogen Whichfgen which comprises effecting *a cyanogen V comprises establishing extended and conm' i in -a mass of inoltencarbon dissolving mamay be effected, by under pressure,'

lterial. to maintainv t v distil outthe"=cyano'gen` compound.Jorinecl,l l f pound.

ling thereon, angl' means for iiutroclucing" v '-Galkali metalr and free'nitr'ogen intoy said' y nitiogento simultaneously reactv upon the 2'O.' `n relectric nitrogen fixing `:furnace the llease of a cyanogen compound .to he Y formed andv free nitrogen into'said molten comprisingy a moltenfhath of carbon dissolving catalytic material, a resistor of carboni fragments, electrically conductive lmeans for orcing a considerable-,partei said resistor down into said molten bath. to supply carbon as Wellas electriccurrent thereto, and means to 'supplyya iiitrogenous and cyanid-base f f ysupplying reagent togsaid `hath-capable of reacting uponkthe; dissolvedcarbon therein to form a cyanogen compound. f

r22. An electric nitrogen gixing furnace comprising a hath of molten 1carbon dissolving'catalyticy materi'al,.means to supply al" gaseous nitrogenous and cyanid-hase. spf plying reagent to rsaid.loatli,anol an electric 80 resistor for said furnace adapted to heat the same and to preventy the too free escape ofv y'said reagent"from said bath.

23.l The process l of 1'ohtai'ning fixed nitrogen which comprises veffecting a ycyanogen ticipate4v the .carbonfdissolved in and Present i throughout a mass' 'of carbondissolving inaterial which fis capable of acting catalyti-A cally in said reactiolliffree 1nitrogen and a vaporadapted to supplythel base of the cyanogen compoundr to yhe --ormed, While in-y troducing-,bothsaid free nitrogen. and vapor into said-mass, electrically `heating saidmaterial. to a temperature suiicient to favor saidreaction and vtoolistil out the cyanogen compound ormedpan'd collecting the'so distilled cyanogen "cc'zinp'ound'.

24; vThe processoiobtaining fixed nitrocompound forming reaction'J-in which par` ticpate 'the v carbon dissolved .in and'present throughout a molten inassofcarbonjdissolvi ing materialvwliich'iscapahleof acting cata- 4lytieally in: said reaction; free nitrogen and a vapoiadapted tQsupply the base of the cjy-anogen compoundtobatormed, While in'- troducing both said free nit'iogengaiid vapor into said massyelectrically 4heating said Ina- 1e` same molten and to and collectingftheso distilled cyanogen comf 25. The processsof obtaining ii'iXed'nitrO-i' genuwhich comprisesy effecting a cyanogen 12o adapted-to supplygthe'basc of the'lcyilnogen l compound to be formed5 while introducin both said Afree nitrogeniand Vapor into"`sai mass, electrically heating Said metal @9"@1125 temperature sufficient to favorsaid reaction* and to distil out thecyanogen. ycompound termed, andV collectingitheso distilled cys` -aiiogen compound.` 26. Theprocessojolataining tixedlnitro-v gen which comprisesjeifecting'a ycyz'iliiogen 130 ,compound 4forming `reactionfiii which particcompound forming reaction` in which par, l`out the cyanogen compound formed, and 110 :tcipate the carbon dissolved in and present throughout a. mass of carburzed iron, free nitrogen and a vapor 'adapted to Supply the base of the eyanogeu compound to be formed,` While introducing both said free nitrogen and vaporjinto said mass, electrically heatingthe iron to a. tempepature sufe'eut to `favor said reaction and to dstil f pound.

collecting the so distilled eyanogen com- 1ntestimo1'1ywhereofl I have afxedmj;

,eignaturg in `the preeenee of two Witnesses.

. JOHN E. BCHER. y, Witnesses: y

-HOWARD C. RIPLEY,

HoWAxgp F. HYLAND. 

